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Ionic conduction in solids that exceeds 0.01 S/cm is predicted to involvecollective phonon-ion interactions in the crystal lattice. Here, we use theoryand experiment to measure the contribution of possible collective phonon-ionmodes to Li+ migration in Li0.5La0.5TiO3. The ab initio calculations revealthat only a few phonon modes, mostly TiO6 rocking modes below 6 Terahertz,provide over 40% of the energy required for the Li+ hop in Li0.5La0.5TiO3.Laser-driving the TiO6 rocking modes decreases the measured impedance ten-foldcompared to exciting acoustic and optical phonons at similar energy densities.The decreased impedance persists on thermalization timescales. These findingsprovide new insights on phonon-coupled ion migration mechanisms, materialdesign rules, and the potential for metastable states for opto-ionic materials.

Correlated Terahertz phonon-ion interactions dominate ion conduction in solid electrolyte Li0.5La0.5TiO3